Photophysics of C60 Colloids
ARMY TANK AUTOMOTIVE RESEARCH DEVELOPMENT AND ENGINEERING CENTER WARREN MI
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The goal of this dissertation is to study the photophysics of suspensions of colloidal C60 particles to determine if their nonlinear optical NLO response is superior in any way to benchmark NLO materials such as molecular solutions of C60 and carbon black suspensions CBS. C60 in molecular form is known to exhibit strong reverse saturable absorption RSA and it is posited that colloidal particles composed of many C60 molecules would maintain some degree of RSA behavior upon association, although some quenching is to be expected. CBS is known to have an NLO response that is dominated by nonlinear scattering resulting from a phase change due to heating of the carbon black particles by absorbed energy. Colloidal C60 particles that are many nanometers in diameter are similar to CBS, so it is posited that they would also have a nonlinear scattering mechanism contributing to their NLO response. Three samples of C60 colloids are characterized by several techniques, along with two carbon black suspensions and one molecular solution of C60. Transmission electron microscopy is used to determine morphology. Femtosecond pump-probe spectroscopy is used to determine the absorption spectrum and the relaxation kinetics of the first excited singlet state. Nanosecond laser flash photolysis is used to determine the absorption spectrum and the relaxation kinetics of the first excited triplet state. Z-scan is used to determine triplet-triplet absorption cross-sections. An experiment is performed to determine the percentage of the input energy that is transmitted, scattered, or absorbed by each sample. Computer modeling is performed to compare the experimental results to theory. Results show that all materials that exhibit nonlinear scattering have a constant extinction coefficient in the nonlinear regime, implying a characteristic size for the scattering centers that is independent of input energy.
- Atomic and Molecular Physics and Spectroscopy